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ZrO2 thin films were deposited by using an electron beam evaporation technique on three kinds of lithium triborate (LiB3O5 or LBO) substrates with the surfaces at specified crystalline orientations. The influences of the LBO structure on the structural and optical properties of ZrO2 thin films are studied by spectrophotometerand x-ray diffraction. The results indicate that the substrate structure has obvious effects on the structural and optical properties of the film: namely, the ZrO2 thin film deposited on the X-LBO, Y-LBO and Z-LBO orients to m(-212), m(021) and o(130) directions. It is also found that the ZrO2 thin film with m(021) has the highest refractive index and theleast lattice misfit.